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Regensburg 2022 – wissenschaftliches Programm

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O: Fachverband Oberflächenphysik

O 35: Poster Tuesday: Plasmonics and Nanooptics 1

O 35.6: Poster

Dienstag, 6. September 2022, 11:00–13:00, P3

Mapping Lamb, Stark and Purcell effects at a chromophore-picocavity junction with hyper-resolved fluorescence microscopy — •Anna Rosławska1, Tomáš Neuman1,2,3, Benjamin Doppagne1, Andrei G. Borisov3, Michelangelo Romeo1, Fabrice Scheurer1, Javier Aizpurua2, and Guillaume Schull11Université de Strasbourg, CNRS, IPCMS, UMR 7504, F-67000 Strasbourg, France — 2Center for Materials Physics (CSIC-UPV/EHU) and DIPC, Paseo Manuel de Lardizabal 5, Donostia - San Sebastián 20018, Spain — 3Institut des Sciences Moléculaires d’Orsay (ISMO), UMR 8214, CNRS, Université Paris-Saclay, 91405 Orsay Cedex, France

Light-matter interaction plays a crucial role in the properties of light emission from single molecules. Here, we show that it can be probed with sub-molecular precision thanks to the atomically-confined electromagnetic field at the scanning tunneling microscope tip apex, which acts as a picocavity for localized plasmons. Such strong fields interact with the molecular exciton via Purcell, Lamb and Stark effects, which enable tuning the emission energy and line width. Hyper-resolved fluorescence maps of these two parameters can be understood as images of the static charge redistribution upon electronic excitation of the molecule, and the distribution of the dynamical charge oscillation associated with the molecular exciton, respectively [1].

[1] A. Rosławska et al., Phys. Rev. X, 12, 011012, 2022.

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